Producing compounds containing carbon and hydrogen.



UNlTED STATES PATENT omen.

ALWIN MITTASCH ANDCHRISTIAN SCHNEIDER, OF- LUZDWIGSHANEN-ON-THE-RHINE,

GERMANY, ASSIGNORS 'IO BADISCHE ANILIN & SODA FABRIK, OF LUDWIGSHAFEN- r ON-THE-RHINE, GERMANY, A. CORPORATION.

PRODUCING COMPOUNDS CONTAINING CARBON AND HYDROGEN.

No Drawing.

To all whom it mag concern: I

Be it known that we, ALWIN MITTASCH and CHRISTIAN SCHNEIDER, citizens of the GermanEni'pire, residing at Ludwigshafenon-the-Rhine, Germany, have invented new.

and useful Improvements in Producing Compounds Containing Carbon and Hydrogen, of which the following is a specifica tion.

It is known that methane can be obtained from carbon monoxid and carbon dioxid and hydrogen at a raised temperature by means of catalytic agents, in particular nickel, and it has also been stated that by altering the conditionsof the experiment small quantities of formaldehyde and ethylene are also sometimes produced.

We have found that a new result can be obtained and that we can build up a number of organic compounds when working under pressure under suitable conditions as hereinafter set forth.

We have found that the compounds containing carbon and hydrogen, including hydrocarbons, (in particular such as are liquid or which can be easily liquefied,) and also oxygen compounds of hydrocarbons can be obtained by passing an oxid of carbon and hydrogen either alone or in admixture with other gases over a heated catalytic agent under a pressure exceeding that of live-atmospheres. According to the nature of the catalytic agent employed and the conditions of working, litferent compounds or mixtures are obtained, for instance, liquid hydrocarbons either saturated or unsaturated, and alcohols, aldehydes, ketones and acids, In order to obtain larger quantities of liquid compounds, it is often advantamium, cobalt, manganese, molybdenum, osmium, palladium, titamum, zlncand oxids or other compounds of these metals and if Specification of Letters latent. P t t g t, 17, 19 6, v

Application filed February 11, 1914. Serial No. 818,054.

Although the advantages of our invention can be obtained by working at a pressure above about 5 atmospheres, we prefer to employ higher pressures ranging say from 20 atmospheres upward.

The temperature of the reaction may, generally, be kept between about 200 to 500 C.

The following examples will serve to illustrate further the nature of our invention, which, however, is not confined to these exam les.

ixample 1: Impregnate pure asbestos with pure cobalt oxid, or osmium oxid, together with a little caustic soda, and then, while employing a coppered iron vessel with steel jacket and working at a pressure of 100 atmospheres and atemperature of from 300400 C. pass over the catalyst thus prepared a mixture containing one part of pure hydrogen, and two or more parts of well as oxygen derivatives of the hydrocarbons, are formed and can be at once condensed or absorbed in a cold receiver. Generally, an aqueous solution of aldehydes and the like isobtained in addition to a light, oily liquid consisting chiefly of saturated and unsaturatedhydrocarbons which boil up to 250 C. or even higher. It is preferred to maintain the receiver under the same pressure as thereaction space and to effect the condensation .by cooling. If desired, a frac-' tionated cooling can be efi'ected either with or without releasing the pressure. A similar procedure can be followed when using carbon dioxid instead of, or in addition to carbon monoxid, more oxygen containing compounds and less hydrocarbons being then obtained.

g Exampe 2: Impregnate a suitable carrier,

for instance, calcined magnesla, pumice, or

diatomite with potassium carbonate solution and then dry the mass and introduce it into a concentrated solution of zinc nitrate, pour off the liquid and dry and heat the contact mass which is then placed in a suitable apparatus; while employing a pressure of 120 atmospheres and a temperature of from 360- 420 0. pass through theapparatussa gas mixture containing 62% of carbon monoxid, 28% of hydrogen, 4% of, carbon dioxid, 2% of methane and 4% of nitrogen. The'products consist chiefly of higher hydrocarbons and derivatives thereof. In this case carbon is generally not deposited or at the most only to a slight extent. The greater part of the products capable ofliquefaction or absorption can be separated at ordinary tempera ture and the remaininggas generally contains olefins, such as ethylene and propylone, and further, paraflins such as methane and ethane. Analysis of the products obtained shows that the oily layer consists chiefly of hydrocarbons. o bo1ling points from 20 to well above 200 C. i For instance, about two-thirds are saturated and the rest olefinic, but this proportion can vary considerably. In addition to these hydrocarbons, organic ox gen compounds of various kinds are contained dissolved in the hydrocarbons. The oily layer, either before or after special purification possesses the character of the natural ethereal oils. Analysis of the aqueous layer showsa varying content of saturated and unsaturated organic compounds consisting, for instance, of alcohols, ketones, (such'as acetone), aldehydes, (such as formaldehyde), acids, (such as acetic acid and higher homologues thereof,) and also other condensation products.

In those cases in which the gas mixture employed is not sufficiently pure, but contains traces of substances deleterious to the reaction, it is preferred to purify the gases specially, for instance, by passing them beforehand at a raised temperature through a purifier containing material similar to that employed as the catalyticagent. The gases leaving the receiver can after correcting their contents, for instance, by removing carbondioxid and adding hydrogen, and the process can be carried out under continuous ressure. j Now what we 0 aim is 1. .The process of producing compounds containing carbon and h dro catalytic agent under a be used over again an oxid of carbon an hy heated catalytic agent under ceeding that of 5 atmospheres.

2. The process of roducing compounds containing carbon anti hydro en by passing an oxid of carbon and by rogen over a heated catalytic agent under a pressure exceeding that of 20 atmospheres.

3, T e process of reducing compounds containing carbon amfhydrogen by passin carbon monoxid and hydrogen over a heated pressure exceeding rogen over a a pressure excompound of a heavy metal and some alkali under a pressure exceeding that of 20 atmospheres.

7..,The process of producing compounds containing carbon and hydrogen by passin hydrogen with anexcess of carbon monoxi over a heated catalytic agent containin a compound of a heavy metal and some "a1 ali en by passing under a pressure exceeding that of 20 atmospheres and at a temperature between 200 and 500 C.

8. The process of producing compounds containing carbon and hydro en by passing an oxid of carbon. and hy rogen over a heated catalytic agent containing cobalt under a pressure exceeding that ofv 20 atmospheres. p L

9. The process of producing compounds containing carbon and hydrogen by passing an oxid of carbon over a heated catalytic agent containing zinc oxidunder a pressure exceeding that of 20 atmospheres.

10. The process of producing compounds containing carbon and hydrogen by passing a gas mixture containing an oxid of carbon and hydrogen and free from substances deleterious to the reaction over a heated catalytic agent under a pressureexceeding that of 20 atmospheres.

11.. The process of producing compounds containing carbon and hydrogen by passing gases containingl an oxid of carbon and hydrogen over a eatedcatalytic agent under a pressure exceeding that of 20 atmospheres, and then separating by means of cooling the liquid compounds which have been'formed, while maintaining a pressure exceeding that of 20 atm0spheres.- 12. The continuous process of producing 5 compounds containing carbon and hydrogen by passing gases containing an oxid of car- .bon and hydrogen overa heated catalyticagent, then separating by means of cooling the liquid compounds which have been 16 formed, then correcting the composition of the remaining gas mixture, and-passing it allow over-the catalytic agent; the whole process being carried out at a pressure exceeding that of 20 atmospheres.

.In testimony whereof we have, hereunto \115 set our hands in the presence of two subscribing witnesses.

' ALWIN MITTASCH. a CHRISTIAN SCHNEIDER. Witnesses: I

J. ALEC.- LLOYD, S.S. BERGER, 

